製備Fe金屬附載於碳化ZIF-67對抗生素與有機染料降解及六價鉻離子還原之催化反應

Please use this identifier to cite or link to this item: http://ir.lib.ncu.edu.tw/handle/987654321/89139

Title:	製備Fe金屬附載於碳化ZIF-67對抗生素與有機染料降解及六價鉻離子還原之催化反應
Authors:	張在焮;Chang, Tsai-Hsin
Contributors:	化學學系
Keywords:	ZIF-67;Fenton;chromium reduction
Date:	2022-07-27
Issue Date:	2022-10-04 10:59:22 (UTC+8)
Publisher:	國立中央大學
Abstract:	本論文研究為合成雙金屬有機金屬骨架材料，並將其碳化應用在催化反應上，使材料中金屬節點還原成金屬態並把有機配體碳化成氮參雜碳材以增加材料穩定度。以2-甲基咪唑與鐵和鈷的前驅物合成Fex-ZIF67，再以高溫鍛燒爐碳化成碳材Fex-CZ67，碳化後材料的穩定性得以提升，並且金屬還原後仍保有催化活性。第一部分實驗中，針對抗生素—四環黴素與有機染料的Fenton降解反應，以調控鈷和鐵的含量達到最佳的降解效果，僅含鈷的CZ-67對四環黴素的降解需經過8.5分鐘才能反應完全，準一級反應速率常數k為42.78（min-1gcat-1）；而Fe0.1-CZ67和Fe0.2-CZ67的k值分別下降至18.98與14.92。但當鐵含量上升至40%時（Fe0.4-CZ67）降解速率為最快，3.5分鐘四環黴素降解率達到94.2%，且反應率速率常數k達到79.54，這個結果歸因於鐵和鈷的協同效應，而鈷可能為主要的催化金屬，所以Fe0.1-CZ67和 Fe0.2-CZ67的鈷含量降低且鐵的含量不足以在此反應產生協同效應。第二部分的實驗為六價鉻還原反應，CZ-67對六價鉻還原需經過135分鐘，準一級反應速率常數k為2.16；而隨著鐵的含量上升至50%（Fe0.5-CZ67）時，7.5分鐘六價鉻還原率達到99.76%，反應速率常數k上升至79.29。此結果歸因於鐵和鈷的協同效應。 ;This thesis is about to synthesize bimetallic metal-organic framework (MOF) materials and carbonized them to apply on catalytic reactions. Carbonization of MOF materials will makes metal nodes in MOF reduce to metallic states, and the organic linkers will also turn into N-doped carbon material to increase the stability of materials. Fex-ZIF67 was synthesized with 2-methylimidazole and precursors of iron and cobalt, and then carbonized into carbon material Fex-CZ67 in a high-temperature calcining furnace. The first part of experiment is the Fenton degradation reaction of antibiotics-tetracycline and organic dyes. To adjust the content of cobalt and iron to achieve the best degradation effect, it takes 8.5min to degrade tetracycline completely by CZ-67, and the pseudo-first-order reaction rate constant k is 42.78 (min-1gcat-1); while the k values of Fe0.1-CZ67 and Fe0.2-CZ67 drop to 18.98 and 14.92, respectively. But when the iron content rises to 40 % (Fe0.4-CZ67) has the fastest degradation rate, the degradation rate of tetracycline reaches 94.2% in 3.5 minutes, and the reaction rate constant k reaches 79.54. This result is attributed to the synergistic effect of iron and cobalt, while cobalt probably the main catalytic metal, so Fe0.1-CZ67 and Fe0.2-CZ67 have reduced cobalt content and insufficient iron content to provide a synergistic effect in this reaction. The second part of the experiment is the reduction reaction of hexavalent chromium. The reduction of hexavalent chromium by CZ-67 takes 135 minutes, and the pseudo-first-order reaction rate constant k is 2.16; when the iron content rises to 50 % (Fe0.5-CZ67) has the fastest reduction rate, the reduction rate of hexavalent chromium reached 99.76% in 7.5 minutes, and the reaction rate constant k increased to 79.29. This result is attributed to the synergistic effect of iron and cobalt.
Appears in Collections:	[Graduate Institute of Chemistry] Electronic Thesis & Dissertation

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